Controlling photophysics and photochemistry via quantum superpositions of electronic states: towards attochemistry

通过电子态的量子叠加控制光物理和光化学:走向原子化学

基本信息

  • 批准号:
    EP/T006560/1
  • 负责人:
  • 金额:
    $ 61.1万
  • 依托单位:
  • 依托单位国家:
    英国
  • 项目类别:
    Research Grant
  • 财政年份:
    2020
  • 资助国家:
    英国
  • 起止时间:
    2020 至 无数据
  • 项目状态:
    已结题

项目摘要

When molecules absorb light of sufficient energy, an excited electronic state is generated. The distribution of electrons - the chemical bonding - then changes, causing the nuclei to move in response. Electronic changes such as these appear to be instantaneous relative to the nuclear motion that follows. We now know that these electronic changes aren't instantaneous, but they are usually much faster than the nuclear motions, which has limited our scope for controlling their effects until now.We propose to explore how laser manipulation of electronic state motion can offer unprecedented control over photochemistry: chemical reactions that are initiated by changes in bonding in electronic excited states. Can we direct the outcome of a photochemical process in a molecule by controlling the initial evolution of a coherent quantum superposition of its electronic states? Our proposed research will explore a new approach to controlling dynamics in molecular systems at an important interdisciplinary junction. It promises to benefit our understanding of - and mastery over - ultrafast chemical processes, and to extend our ability to manipulate quantum states of matter into the attosecond time domain.Recently attosecond molecular physics has been exploring the concept of "charge migration": electronic dynamics following sudden excitation of an electron in a molecule or other extended quantum system. To understand such phenomena we must recognise the quantum nature of both electrons and nuclei. Ultrafast decoherence due to coupling of the evolving electronic and nuclear quantum states is found to be rapid and general, taking place on a timescale of a few tens of femtoseconds. The control of photoexcited quantum state dynamics can therefore only be achieved with light fields applied on a faster timescale, before decoherence removes our scope for control. A central target of this research is the control of quantum evolution by ultrafast light fields in the vicinity of conical intersections: molecular geometries where crossings between electronic states can lead to multiple chemical pathways. Control here will give us control over different chemical outcomes. Excitation-control-probe sequences of light pulses will be applied to selected molecules. A few-femtosecond UV excitation pulse will initiate the electronic state superposition, followed by a few-cycle infrared pulse after a short and precisely controlled time delay. This pulse sequence will manipulate the coherence between states as the system flows through the critical conical intersection. By varying the superposition within a time interval of a few tens of femtoseconds in this way - on a time-scale faster than decoherence - we will change the quantum evolution path and final outcomes. This path will be measured in real-time via X-ray spectroscopy with sub-femtosecond X-ray pulses, a technique with a high sensitivity to molecular structure and electronic states. Computer simulations using state-of-the-art codes and substantial computing power to solve the coupled electronic-nuclear motions will be used both to predict and to explain the experiments.We will study the dynamics and control of small, isolated, molecular systems in this proposal. Nevertheless, it is likely that what we will learn through this research will be applicable to the quantum scale manipulation of many other light-absorbing systems with ultrafast chemical dynamics. This work is therefore pertinent to a wide range of nanoscale systems: nanoparticles, catalytic complexes, biomolecules, organic optoelectronics, two-dimensional materials and other advanced materials. As well as providing new insight into the fundamental behaviour of molecules, the ultrafast quantum science we are researching may lead to future quantum devices where the flow of charge, energy and information within a quantum system can be controlled by ultrafast light fields.
当分子吸收足够能量的光时,产生激发电子态。电子的分布--化学键--然后发生变化,导致原子核相应地移动。这样的电子变化相对于随后的核运动来说似乎是瞬时的。我们现在知道这些电子的变化不是瞬时的,但它们通常比核运动快得多,这限制了我们迄今为止控制它们的影响的范围。我们打算探索激光操纵电子态运动如何能够提供对光化学的前所未有的控制:化学反应是由电子激发态中的键合变化引发的。我们能否通过控制一个分子的电子态的相干量子叠加的初始演化来指导分子中光化学过程的结果?我们提出的研究将探索一种新的方法来控制分子系统中的动力学在一个重要的跨学科的交界处。它有望帮助我们理解和掌握超快化学过程,并将我们操纵物质量子态的能力扩展到阿秒时间域。最近阿秒分子物理学一直在探索“电荷迁移”的概念:分子或其他扩展量子系统中电子突然激发后的电子动力学。为了理解这种现象,我们必须认识到电子和原子核的量子性质。由于电子和核量子态的耦合,超快退相干被发现是快速和普遍的,发生在几十飞秒的时间尺度上。因此,在退相干消除我们的控制范围之前,光激发量子态动力学的控制只能通过在更快的时间尺度上施加光场来实现。这项研究的一个中心目标是通过圆锥形交叉点附近的超快光场控制量子演化:电子态之间的交叉可以导致多种化学途径的分子几何结构。控制这里将使我们控制不同的化学结果。光脉冲的激发-控制-探测序列将被应用于选定的分子。几个飞秒的紫外激发脉冲将启动电子态叠加,随后是几个周期的红外脉冲后,短和精确控制的时间延迟。当系统流经临界圆锥交叉点时,该脉冲序列将操纵状态之间的相干性。通过以这种方式在几十飞秒的时间间隔内改变叠加-在比退相干更快的时间尺度上-我们将改变量子演化路径和最终结果。这一路径将通过X射线光谱学与亚飞秒X射线脉冲进行实时测量,这是一种对分子结构和电子状态具有高灵敏度的技术。计算机模拟使用最先进的代码和大量的计算能力来解决耦合的电子-核运动将被用来预测和解释实验。我们将研究小的,孤立的,分子系统的动力学和控制在这个建议。尽管如此,我们通过这项研究所学到的东西很可能适用于许多其他具有超快化学动力学的光吸收系统的量子尺度操纵。因此,这项工作与广泛的纳米系统有关:纳米颗粒,催化复合物,生物分子,有机光电子学,二维材料和其他先进材料。除了提供对分子基本行为的新见解外,我们正在研究的超快量子科学可能会导致未来的量子设备,其中量子系统内的电荷,能量和信息的流动可以由超快光场控制。

项目成果

期刊论文数量(7)
专著数量(0)
科研奖励数量(0)
会议论文数量(0)
专利数量(0)
Quantum Interference Paves the Way for Long-Lived Electronic Coherences
量子干涉为长期电子相干性铺平了道路
  • DOI:
    10.1103/physrevlett.129.173203
  • 发表时间:
    2022
  • 期刊:
  • 影响因子:
    8.6
  • 作者:
    Dey D
  • 通讯作者:
    Dey D
Control of nuclear dynamics in the benzene cation by electronic wavepacket composition.
  • DOI:
    10.1038/s42004-021-00485-3
  • 发表时间:
    2021-04-01
  • 期刊:
  • 影响因子:
    5.9
  • 作者:
    Tran, Thierry;Worth, Graham A.;Robb, Michael A.
  • 通讯作者:
    Robb, Michael A.
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Graham Worth其他文献

Graham Worth的其他文献

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{{ truncateString('Graham Worth', 18)}}的其他基金

A Universal Approach for Solving Real-World Problems Using Quantum Dynamics: Coherent States for Molecular Simulations (COSMOS)
使用量子动力学解决现实世界问题的通用方法:分子模拟的相干态 (COSMOS)
  • 批准号:
    EP/X026973/1
  • 财政年份:
    2023
  • 资助金额:
    $ 61.1万
  • 项目类别:
    Research Grant
Rational design of photoactive molecules using "black box" quantum dynamics simulations
使用“黑匣子”量子动力学模拟合理设计光活性分子
  • 批准号:
    EP/S028781/1
  • 财政年份:
    2019
  • 资助金额:
    $ 61.1万
  • 项目类别:
    Research Grant
Developing the MCTDH Quantum Dynamics Code: Accurate Direct Dynamics of Non-Adiabatic Phenomena
开发 MCTDH 量子动力学代码:非绝热现象的精确直接动力学
  • 批准号:
    EP/K037943/2
  • 财政年份:
    2016
  • 资助金额:
    $ 61.1万
  • 项目类别:
    Research Grant
Photoelectron spectroscopy in a liquid microjet: unravelling the excited state dynamics of photoactive proteins
液体微射流中的光电子能谱:揭示光活性蛋白质的激发态动力学
  • 批准号:
    EP/L005697/2
  • 财政年份:
    2016
  • 资助金额:
    $ 61.1万
  • 项目类别:
    Research Grant
CCPQ: Quantum Dynamics in Atomic, Molecular and Optical Physics
CCPQ:原子、分子和光学物理中的量子动力学
  • 批准号:
    EP/M022544/2
  • 财政年份:
    2016
  • 资助金额:
    $ 61.1万
  • 项目类别:
    Research Grant
CCPQ: Quantum Dynamics in Atomic, Molecular and Optical Physics
CCPQ:原子、分子和光学物理中的量子动力学
  • 批准号:
    EP/M022544/1
  • 财政年份:
    2015
  • 资助金额:
    $ 61.1万
  • 项目类别:
    Research Grant
Photoelectron spectroscopy in a liquid microjet: unravelling the excited state dynamics of photoactive proteins
液体微射流中的光电子能谱:揭示光活性蛋白质的激发态动力学
  • 批准号:
    EP/L005697/1
  • 财政年份:
    2014
  • 资助金额:
    $ 61.1万
  • 项目类别:
    Research Grant
Developing the MCTDH Quantum Dynamics Code: Accurate Direct Dynamics of Non-Adiabatic Phenomena
开发 MCTDH 量子动力学代码:非绝热现象的精确直接动力学
  • 批准号:
    EP/K037943/1
  • 财政年份:
    2013
  • 资助金额:
    $ 61.1万
  • 项目类别:
    Research Grant
Wavepacket dynamics for the future: A general purpose HPC-compliant program.
面向未来的 Wavepacket 动力学:通用 HPC 兼容程序。
  • 批准号:
    EP/G055270/1
  • 财政年份:
    2009
  • 资助金额:
    $ 61.1万
  • 项目类别:
    Research Grant
Stark shifting the barrier to reaction: Control through using a strong laser field to shape the potential energy surfaces
彻底改变反应障碍:通过使用强激光场塑造势能面进行控制
  • 批准号:
    EP/G014124/1
  • 财政年份:
    2008
  • 资助金额:
    $ 61.1万
  • 项目类别:
    Research Grant

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  • 批准号:
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潜在有用材料的光物理学和光化学
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光活性材料的开发:合成、光化学和光物理学
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潜在有用材料的光物理学和光化学
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通过电子态的量子叠加控制光物理和光化学:走向原子化学
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    $ 61.1万
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“多原子分子的光物理学、光化学和光谱学”
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蓝藻色素 Slr1393g3 光物理学和光化学的分子理解
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